Research Article

Cite This: ACS Appl. Mater. Interfaces 2018, 10, 39942−39951 www.acsami.org

Transparent Tunable Acoustic Absorber Membrane Using Inkjet-

Printed PEDOT:PSS Thin-Film Compliant Electrodes
Milan Shrestha,†,‡ Zhenbo Lu,§ and Gih-Keong Lau*,†
†
School of Mechanical and Aerospace Engineering and ‡Singapore Center for 3D Printing (SC3DP), Nanyang Technological
University, Singapore 639798
§
Temasek Laboratories, National University of Singapore, Singapore 117411
*
S Supporting Information
See https://pubs.acs.org/sharingguidelines for options on how to legitimately share published articles.

ABSTRACT: Window glasses can block noise from outdoor,

Downloaded via NATL CHIAO TUNG UNIV on September 13, 2020 at 15:12:10 (UTC).

but they reverberate sound within a large indoor space.

Microperforated glass absorbers have been developed to
absorb sound over a fixed but narrow bandwidth. To tune the
frequency spectrum of acoustic absorption, we developed a
transparent tunable acoustic absorber based on micro-
perforated dielectric elastomer actuator (MPDEA) and
transparent compliant electrodes. Such transparent compliant
electrodes were inkjet printed from Triton X-plasticized
poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate)
ink, which shows improved wettability on the acrylate dielectric elastomer substrate. These transparent polymeric electrodes
are softer with uptake of moisture while being self-clearable and durable. A single layer of MPDEA using two inkjet-printed
electrodes is 78.64% clear, but the clarity of a two-layer MPDEA decreases to 61.8%. Among the two designs, the two-layer
MPDEA exhibits a broader acoustic absorption bandwidth of 444 Hz for absorbing more than 80% of the sound energy.
Inactivated resonant frequency of this MPDEA is 1170 Hz, whereas the 6 kV activation can reduce the resonant frequency for
15.2% by causing 9% hole-diameter contraction. This transparent tunable acoustic absorber can be fitted to window glass; its
acoustic performance is better than that of translucent curtains.
KEYWORDS: PEDOT, PSS, inkjet printing, acoustic absorber, transparent compliant electrodes, dielectric elastomer actuator

1. INTRODUCTION membrane absorbers.20−22 In addition, the same actuation

Glass panels are widely used to cover windows of shops and
offices. They are optically transparent to allow daylighting, but
they reverberate sound within a large indoor space. For
example, in a restaurant where windows were closed,
conversation among diners can reverberate indoor and thus
turn more noisy1 than where windows were opened. There are
a few solutions for sound absorption and being optically clear.
Curtains are often used for interior acoustic absorption, but
they are usually opaque for view. A translucent woven fabric,
i.e., Gerriets Absorber Light,2 is recently developed for sound
absorption while allowing natural lighting. Meanwhile, micro-
perforated glass panels3−9 were proposed to be installed to
window; their acoustic absorption spectrum is however fixed
and not as broad as fabric absorber.10,11
Active tuning of a panel absorber can help shift the acoustic
absorption spectrum to target varying noise. Electroactive
polymers12−18 provide a silent means of distributed actuation,
being much lighter than conventional servo motors. Recently,
dielectric elastomer actuators (DEAs) have been used to make
for tunable acoustic absorbers.19−21 A dielectric elastomer
actuator is a soft capacitor that consists of a prestretched
dielectric elastomer membrane sandwiched between a pair of
compliant electrodes. It was used to reduce the membrane
tension and thus shift the acoustic resonant frequency of the
principle can control the hole size of a microperforated
dielectric elastomer membrane for tunable bands of acoustic
absorption.23 These tunable acoustic absorbers developed so
far are opaque due to the use of carbon-based20,21 or gold-thin-
film compliant electrodes23,24 for dielectric elastomer actuators.
For window use, a tunable acoustic absorber based on DEA
requires transparent compliant electrodes.25 Inkjet printing
techniques promise being handy for complex patterning of
conductive ink, but the uniform printing of a submicron thin
film is challenging on the slightly hydrophobic surface of
acrylic elastomer substrate.
Common electrode materials for dielectric elastomer
actuators include conductive grease (such as carbon grease
or silver grease),12,13 conductive powders (such as carbon
black or graphite powder),26,27 and conductive nanometric
networks (such as carbon nanotubes or silver nanowires).28,29
Among them, a sparse and smooth coverage of conductive
nanometric network,29 such as carbon nanotube, is transparent
on dielectric elastomer actuators. However, this initially
transparent DEA turns hazy upon activation.28,30 The haze
Received: July 21, 2018
Accepted: October 26, 2018
Published: October 26, 2018

© 2018 American Chemical Society 39942 DOI: 10.1021/acsami.8b12368

ACS Appl. Mater. Interfaces 2018, 10, 39942−39951
ACS Applied Materials & Interfaces Research Article

Figure 1. Transparent tunable acoustic absorber based on microperforated dielectric elastomer actuator (MPDEA): (a) schematic showing the
device components; (b, c) a unit cell at inactivated and activated states; and (d) measurement setup with an acoustic impedance tube.

Figure 2. Modulus determination of plasticized PEDOT:PSS nanometric films by tensile testing: (a) schematic for a sample consisting of a
uniaxially prestretched VHB tape (F9473PC) sandwiched between two plasticized PEDOT:PSS nanometric films. (b, c) Surface morphology of
plasticized PEDOT:PSS nanometric film at 0% strain (L0 = 10 mm) and 15% strain (L = 15 mm). (d) Tension required to stretch the sample
starting with a relaxed thin film (L−20 mm) and above. (e) Tensile stress as extracted from the extra force to stretch the PEDOT:PSS nanometric
films.

happens because the surface of dielectric elastomer roughens
when electrostatically squeezed (or indented) by the networks
of conductive nanotubes or nanowires.30 Hydrogel or ionic gel
(which was swollen by ionic liquids)31,32 can remain
transparent during large-strain activation and deactivation of
dielectric elastomer actuator. However, the gel is prone to dry
up and the dried patch appears whitish due to residue salt.33−35
Liquid encapsulation can help preserve moisture,35−37 but it is
prone to leakage.
Poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate)
(PEDOT:PSS) has been widely used as a transparent
conductive coating of antistatic shielding bag38 and a
transparent polymeric conductor for all-polymer capacitors,39
transistors,40,41 or solar cells.42 Nanometric film of PE-
DOT:PSS also makes a stretchable electrode on a hyperelastic
substrate of elastomer membrane.43,44 Conductivity of the
PEDOT:PSS film is higher than that required by compliant
electrodes for dielectric elastomer actuators. In addition, the
stretched film of PEDOT:PSS is prone to plastic yielding
39943
beyond 2% strain.45 When stretched uniaxially beyond 30%
strain,43 the PEDOT:PSS film is prone to crack and lose
conductivity.
Being moderately stretchable, nanometric films of PE-
DOT:PSS are good enough as compliant electrodes for
moderate-strain actuation of dielectric elastomer. Previously,
pristine PEDOT:PSS was not applied as compliant electrodes
because the former’s modulus of 2GPa43,45 is 4 orders higher
than the 0.2−0.5 MPa modulus of acrylate dielectric
elastomer.46,47 This suggests that even a submicron thin film
of PEDOT:PSS is axially stiffer than a hundred-micron
membrane of acrylate elastomer (e.g., VHB 4910). Further-
more, the aqueous ink of pristine PEDOT:PSS does not spread
well on the slightly hydrophobic surface of acrylate dielectric
elastomer. Recently, Yoon et al.48 reported the addition of
surfactant Triton X-100 improved the wettability of aqueous
suspension of PEDOT:PSS on a polydimethylsiloxane
elastomer substrate while acting as a plasticizer to soften the
obtained solid film of PEDOT:PSS. The modulus of plasticized
DOI: 10.1021/acsami.8b12368
ACS Appl. Mater. Interfaces 2018, 10, 39942−39951
ACS Applied Materials & Interfaces
Figure 3. (a) Fabrication steps for making a MPDEA: (1) substrate preparation by prestretching a VHB tape; (2) inkjet printing of PEDO:PSS thin
film on the substrate; (3) inkjet printing on the other side; (4) heating of printed ink droplets in an oven; (5) laser drilling to make holes through
the substrate membrane; (b) evolution of print in side and top views: from (b(2)) wet droplets, (b(2b)) merged puddles, to (b(4)) dried solid thin
film.
PEDOT:PSS was not directly measured but only inferred from
buckling mechanics of a thick elastomer substrate.48,49
Motivated by this recent finding, we shall re-examine the
feasibility and formulation of PEDOT:PSS for making
compliant electrodes of dielectric elastomer actuators.
In this work, we developed a transparent tunable acoustic
absorber (see Figure 1) based on a microperforated dielectric
elastomer actuator with inkjet-printed transparent polymer
electrodes. Here, we formulated a plasticized and diluted ink of
PEDOT:PSS with reduced modulus and improved wettability
on elastomeric substrate. Such inkjet-printed transparent
polymeric thin films can make compliant electrodes for driving
a dielectric elastomer actuator for up to 20.6% radial strain,
whereas ductile fracture happens above 15%. In addition, the
DEA with such transparent compliant electrodes are self-
clearable from dielectric breakdown and durable to withstand
actuation cycles and humidity changes. A microperforated
dielectric elastomer actuator (MPDEA) with the inkjet-printed
compliant electrode can tune the acoustic absorption spectrum
while transmitting light. Such a transparent acoustic absorber
will suit to be fit to window glass.
2. METHODS AND MATERIALS
Figure 1a−c shows a transparent tunable acoustic absorber consisting
of a microperforated dielectric elastomer actuator (MPDEA), a rigid
ring frame, and a back cavity plate, all in a circular outer profile. Being
a soft capacitor, a MPDEA consists of a microperforated membrane
(MPP) of a dielectric elastomer sandwiched between a pair of
transparent polymeric compliant electrodes. The back cavity of
acoustic absorber is formed as the air spacing between the MPDEA
membrane and the back plate of acrylic, which can be replaced by a
window glass panel. Subsequent subsections present the working
principle and design of dielectric elastomer actuator, design of
compliant electrodes, Helmholtz resonator design, device fabrication,
inkjet printing, and experimental setup.
2.1. Dielectric Elastomer Actuator. Dielectric elastomer
actuator (DEA) is a soft capacitor capable of producing deformation
or tension change under electrostatic pressure (Maxwell stress).12,13
39944
Research Article
Typically, it consists of a biaxially prestretched dielectric elastomer
membrane sandwiched between a pair of compliant electrode.
Application of high voltage V across the dielectric membrane of
thickness ts induces a compressive electrostatic pressure pe = ϵrϵ0(V/
ts)2, where ϵr is the dielectric constant and ϵ0 is the permittivity of
vacuum.12,15 This activation reduces the biaxial pre-tension T0 in the
membrane by ΔT(V) such that the membrane tension reduces to
ν
T = T0 − ΔT (V ) = T0 − p
1−ν e (1)
where ν is the Poisson’s ratio of the dielectric elastomer membrane,
according to ref50 on the assumption of small elastic strain. Maximum
electrostatic pressure is limited to sub-megapascal due to dielectric
breakdown.51,52
Figure 1a−c shows a microperforated dielectric elastomer actuator.
Microperforation or puncturing a hole can locally release the pre-
tension in a membrane, which was not perforated. This leads to the
enlargement of initial puncture size (more than that initially drilled by
laser). Activation of the annular dielectric elastomer actuator that
surrounds the passive hole can reduce the hole radius by Δa(V)
ÅÄÅ ÑÉ
following ref 23
Å ij a2 yzÑÑ
Δa(V ) = ΔT (V )ÅÅÅÅb + − 2a − νjjjb − zzzÑÑÑÑ
ÅÅ j b z{ÑÑÑÖ
a2
ÅÇ b k (2)
where b is the half pitch between holes (see Figure 1b,c).
2.2. Design of Compliant Electrodes. For driving a dielectric
elastomer membrane for large voltage-induced deformation, com-
pliant electrodes must be axially softer than the elastomer substrate;
otherwise, they will limit the deformation.53 Whereas wrinkled
nanometric thin film can be compliant,24,54 thickness control for
nanometric film deposition can be difficult, except by vapor
deposition method. Inkjet printing does not yield high film uniformity
due to the coffee ring effect. To mitigate the impact of thickness
variation, we proposed to formulate the ink recipe to yield a softer
solid conductive film of submicron thickness.
Let us design the modulus of plasticizer-added conductive ink to be
at least 2 times softer than the elastomer substrate. Consider an
acrylate elastomer substrate (3M VHB 4910) with Young’s modulus
Es = 220 kPa and membrane thickness ts = 125 μm, a conductive film
DOI: 10.1021/acsami.8b12368
ACS Appl. Mater. Interfaces 2018, 10, 39942−39951
ACS Applied Materials & Interfaces
of thickness tf = 0.3 μm needs to have a Young’s modulus Ef lesser
than
ts 125 μm
Ef = Es × = 220 kPa × = 45.84 MPa
2tf 0.3 μm (3)
A solid film of 2% Triton X-100/98% PEDOT:PSS was reported48
with a Young’s modulus of 80−92 MPa, as calculated from the
wrinkle mechanics of a PEDOT:PSS-coated elastomer substrate.48
The modulus of the PEDOT:PSS based on this recipe is however
twice stiffer than required. To further soften the electrodes, we need
to add more than 3% Triton X-100 (as a plasticizer) to the conductive
ink of PEDOT:PSS while ensuring the uniformity of printed film on
the VHB substrate.
Here, the conductive ink used for inkjet printing is an aqueous
suspension of PEDOT:PSS. The pristine ink of PEDOT:PSS as
purchased from Clevios P Jet HC V2 from Heraeus Deutschland
GmbH & Co. KG cannot properly wet a slightly hydrophobic surface
of elastomer.44,48 O2 plasma treatment does not make the substrate of
acrylate dielectric elastomer more hydrophilic as it does the silicone
dielectric elastomer.43,44 Hence, the ink needs to be formulated by
adding a surfactant (Triton X-100)48 to improve the wettability on
the elastomeric substrate. The ink was also diluted with deionized
water to yield a thinner solid coating upon drying. Later processes are
based on an optimized formulation consisting of 40.78% weight
PEDOT:PSS ink, 4.5% Triton X-100, and 54.72% deionized water.
A nanometric thin film of plasticized PEDOT:PSS is tacky and
difficult to be released from an elastomer substrate, unlike the release
of pristine PEDOT:PSS film.49 Furthermore, its axial stiffness is low
relative to that of a thick elastomeric substrate. Here, we extract the
modulus of PEDOT:PSS nanometric film from its stiffening effect on
a soft substrate. To pronounce the stiffening effect, a pair of 230 nm
thick plasticized PEDOT:PSS nanometric films were applied to
sandwich a thin and soft substrate of acrylic adhesive tape (VHB
F9473PC) of an 200 μm initial thickness. This sample of a double-
coated tape was bound and clamped by two pairs of 50 mm wide rigid
plates. Figure S1 shows the fabrication steps for making such a tensile-
test sample. The elastomeric substrate was uniaxially prestretched for
two times, whereas PEDOT:PSS films were cast by a doctor blade and
dried on both sides of the substrate through each stencil 50 mm wide
and 10 mm long. A tensile tester (Instron 5569) with a 10N load cell
was used for measuring the tension required to stretch the sample.52
During the tensile test, the sample was stretched from a length of 8
mm to 15 mm. This starting length of 8 mm keeps the VHB tape (of
initial 5 mm length) in tension but causes surface buckling to the
plasticized coatings. Figure 2 shows that the plasticized PEDOT:PSS-
coated VHB tape requires more tension to be stretched as compared
to the noncoated VHB tape. Its first 2 mm extension requires a low
tension to overcome the low elastic resistance of elastomeric tape with
buckled coatings. However, its extension beyond 2 mm sees a marked
increase in the tension requirement to overcome the extra stiffness of
taut coatings. In this way, Young’s modulus of the plasticized
PEDOT:PSS coatings is determined to be 43.1 MPa at room
temperature and 57% relative humidity. Also noted is the yield and
crack formation above uniaxial 15% strain in the overstretched film of
plasticized PEDOT:PSS. Thereafter, the apparent modulus (i.e.,
gradient of tension with respect to stretch) of the VHB with cracked
coating becomes close to that of a pristine VHB tape.
2.3. Helmholtz Resonator Design. A microperforated mem-
brane acoustic absorber is an array of Helmholtz resonators that share
a common back cavity (see Figure 1b,c). A Helmholtz resonator is a
container or cavity of air with a neck-like open hole.10,11,55 When
disturbed by sound, mass of the air plug resonates while compliance
of the back-cavity air provides a restoring force. This resonant
vibration of air can dissipate acoustic energy into heat. According to
ref 55, the fundamental resonant frequency of air-plug vibration in a
Helmholtz resonator is given as
c A
f=
2π SL (4)
39945
Research Article
where c is the sound speed, e.g., 346 m/s, A and L are the cross-
sectional area and the length of the neck-like open hole, respectively,
and S is the volume space of the back air cavity. A back cavity of
radius R and depth H has a total volume space of S = πR2H. Here, a
dielectric elastomer actuator is used to electrically tune the membrane
thickness t = t(V) and tension according to eq 1. Hence, the hole
cross-sectional area A = A(V) = πa2(V) is electrically tunable
following the hole size given in eq 2.
Consider a design of microperforated membrane (MPP) acoustic
absorber with a back cavity of 2R = 20 mm total diameter and H = 40
mm depth. This membrane of t = 250 μm thickness is micro-
perforated with an array of 9 holes of 2a = 540 μm diameter each. For
this MPP, a representative unit of Helmholtz resonators has one ninth
the volume of back cavity and the upper bound of resonant frequency
is estimated to be f = ca /(6πR Ht ) = 1406.45 Hz . Resonant
frequencies of the MPP could be lower, with a larger effective
volume of back cavity. For exact relationship of acoustic character-
istics, please refer to the impedance analysis of a microperforated
panel absorber as presented in the literature.10,11,23,56
2.4. Device Fabrication. Figure 3 shows the fabrication steps for
making a MPDEA, in a similar way to make a soft capacitor. First, an
adhesive tape of acrylate dielectric elastomer (VHB 4910) was
prestretched radially for three times to have a 125.0 μm membrane
thickness, as measured by a micrometer. The measured membrane
thickness is more than the calculated value of 1000 μm/(3 × 3)
because the membrane’s free edges relax and are stretched lesser than
the stretcher with 9 contact points does. Later, the prestretched
membrane was transferred and adhesively bonded to a rigid ring
frame of 20.5 mm internal diameter and 28.0 mm external diameter.
The prestretched elastomer membrane was left for 24 h to relax and
let the viscoelastic creep settle to the steady-state deformation.
Second, aqueous conductive ink of PEDOT:PSS suspension was
inkjet printed on the substrate of the prestretched membrane. Printing
on both sides of the substrate and subsequent drying yield a pair of
transparent polymeric compliant electrodes sandwiching the dielectric
elastomer membrane. Figure 1a shows a circular electrodes of 20 mm
diameter printed on a VHB substrate, except 9 uncoated minor disk
areas within it. These 9 uncoated disk area were arranged in an
orthogonal array with equal spacing of 2b = 5 mm. This distance 2b
between sub-millimeter holes was designed to achieve an open ratio of
less than 1%, following our previous design of opaque MPDEA.23
This membrane DEA can be stacked up readily to another to make a
multilayered membrane DEA. Finally, a laser cutting machine (Epilog
Helix 24) was used to laser drill through the noncoated membrane
areas to produce a microperforated DEA (MPDEA). The average
diameter of the laser drilled holes is 2a = 447.5 ± 30.78 μm for one-
layer MPDEA and 2a = 541.0 ± 25.39 μm for two-layer MPDEA.
2.5. Inkjet Printing of Conductive Ink. A commercial material
printer (Dimatrix 2381)57,58 was used to inkjet print the aqueous
conductive ink. The printhead (cartridge) has 16 nozzles (see Figure
S2); each nozzle can eject an ink droplet of 10 pL. The material
printer can eject conductive ink droplets to form an isolated dot, a line
out of sequential dots with partial overlaps, or an area out of
sequential lines with partial overlaps. To form a continuous film, the
print drop of diameter D needs to be properly spaced with partial
overlap. Figure 3 shows that a proper overlap during printing can
merge wet ink droplets by reflowing into a thin puddle. However, an
insufficient overlap between print dots leads to a void area none-
coated by the wet film; too much overlap yields a thicker puddle.
Baking of the printed wet film in an oven at 50 °C evaporates the
water content of the ink and leaves a solid nanometric film on the
substrate. Transparency of the PEDOT:PSS solid film decreases with
increasing film thickness.
To save printing time, all 16 nozzles of the printhead were selected
for droplet ejection. Typically, inkjet printing of a 20 mm diameter
PEDOT:PSS takes 15−20 min, with all 16 nozzles selected.
Continuity of a printed line/film may be disrupted when some of
the nozzles incidentally c log despite automated nozzle cleaning once
for every printing of 5 lines. Discontinuity in printed line can be
mitigated by using a closer drop spacing. A print drop spacing is
DOI: 10.1021/acsami.8b12368
ACS Appl. Mater. Interfaces 2018, 10, 39942−39951
ACS Applied Materials & Interfaces Research Article

Figure 4. Effect of humidity on properties of plasticized PEDOT:PSS nanometric film: (a) setup for electrical resistance measurement; (b)
humidity effect on electrical resistance; and (c−e) humidity effect on voltage-induced diameter expansion.

Figure 5. Formulation of aqueous PEDOT:PSS ink for improved wettability and formation of uniform and clear film on the VHB substrate: (a)
wettability of ink droplet and uniformity of wet film printed (at 10 μm drop spacing) on the VHB substrate; and (b) effect of ink formulation on
electrical resistance, uniform film formation, and optical transmittance (at 10 μm print drop spacing).

controlled by tilting the printhead relative to the print direction.
According to the printer manual,57 a 10 μm drop spacing is achieved
by a tilt angle of 2.3°, whereas 15 and 20 μm drop spacings can be
obtained at the angles of 3.4 and 4.5°, respectively.
Though this prototype with an inkjet-printed electrode is relatively
small in area, it can be scaled up to be as large as a window glass.
Electrode printing over a large area is possible using industrial
material printers, which have been developed for manufacturing
organic light-emitting diodes display.58−60
2.6. Experimental Setup. Figure S3 shows a high voltage supply
(Trek 610E) being used to activate dielectric elastomer actuators. A
computer and a NI data logger were used to monitor the voltage and
current supplied during the device activation. Gain of the monitor
voltage is one thousandth of the applied high voltage. Meanwhile, a
multimeter (Agilent 34410A) was used to measure the current leaking
through the DEAs and resistance of the electrode.
A camera was used to take the video or pictures of the device in
action, i.e., voltage-induced diameter expansion. A stereoscopic
microscope (Olympus SZX7) was used to have a zoom-in view of
the voltage-induced hole contraction. Images were taken at increasing
voltage steps. Image J software was used to extract the size change
from the images captured.
A confocal microscope (VK-X200 Series 3D Laser Scanning
Confocal Microscope) was used to measure the three-dimensional
(3D) morphology of the printed thin films. This topography
measurement yields the information about the ink dot thickness
and line width.
Figure 1d shows an acoustic impedance tube being used to measure
the acoustic absorption spectrum of a tunable absorber at normal
incidence. The 500 mm long and 20 mm diameter tube has a
loudspeaker installed at one end and the tunable absorber mounted at
the other end. Two electret array microphones (PCB piezotronic,
model 130E20) were used to measure the sound pressures in the tube,

39946 DOI: 10.1021/acsami.8b12368

ACS Appl. Mater. Interfaces 2018, 10, 39942−39951
ACS Applied Materials & Interfaces Research Article

Figure 6. Topography and height measurement for (a) a dot and (b) a line (printed at 10 μm drop spacing); (c) effect on the line width and
thickness; and (d, e) contour plots of printed line topography at 20 and 10 μm drop spacings, respectively.

Figure 7. Inkjet-printed films of PEDOT:PSS on VHB substrate: (a) top-view micrographs showing the effect of print drop spacing; (b) a
photograph showing a setup for resistance measurement; (c, d) effect of drop spacing on electrical sheet resistance and specular optical
transmission (Tspec); and (e) topography and height measurements of a film of PEDOT:PSS printed at 10 μm drop spacing.

namely, pi and pr of incident and reflected sound waves, respectively.

According to ref 61, the sound absorption coefficient (α) is calculated
as 1 − |pr/pi|2. At a 20 mm distance between them, the two
microphones can measure the sound pressure down to 200 Hz.
During the acoustic testing, a data logger NI PXI 6221 was used for
data recording, whereas a high-voltage amplifier (Trek model 20/
20C) was used for driving a device of MPDEA.
Figure S4 shows a spectrometer from AvaSpec (USB2 Fiber Optic)
being used to measure the inline transmittance of a transparent
MPDEA. A halogen light source was used to generate a collimated
light through a 6 mm diameter collimator lens. An optical-fiber
photodetector with a collimator lens was used to detect the specular
light transmitted through the device, which is located at a distance of
70 mm from the collimated lens.

3. RESULTS AND DISCUSSION

It is well known that electrical and mechanical properties of
PEDOT:PSS film change when the conductive polymer takes
up moisture.45,62 This motivated our investigation into the
durability of plasticized PEDOT:PSS nanometric film in the
presence of relative humidity change. The sample under test is
a dielectric elastomer actuator sandwiched between a pair of 20
mm diameter circular compliant electrodes of plasticized
PEDOTP:PSS cast as described above. In this test, we measure
the electrode resistance and dielectric elastomer actuation,
whereas the relative humidity in a humidity chamber changes
between high (80%) and low (25%) at room temperature (25
°C). Figure 4a,b shows that resistance of a plasticized
PEDOT:PSS electrode rises upon drying but decreases upon
39947
Figure 8. Effect of print drop spacing on dielectric elastomer
activation (DEA) and electrode stretchability: (a, b) photographs
showing deactivation and activation (see Movie S1) of a DEA with
PEDOT:PSS electrodes printed at the 15 μm drop spacing; (c, d)
surface topography transition from smooth (before activation) to
microridged (upon release from 10 kV activation); (e) voltage-
induced areal expansion; and (f) leakage current across the dielectric
elastomer upon activation by a stepwise voltage ramp.
moisture uptake. Whereas this moisture-induced resistance
changes by 8.3%, the resistance value of the plasticized
DOI: 10.1021/acsami.8b12368
ACS Appl. Mater. Interfaces 2018, 10, 39942−39951
ACS Applied Materials & Interfaces
Figure 9. Optical clarity of microperforated dielectric elastomer
actuators (with PEDOT:PSS electrodes printed at the 15 μm drop
spacing): (a) a photography of a two-layer MPDEA, which is placed
in front of a black-and-white printed USAF target. (b) Effect of the
number of layer on specular optical transmittance Tspec.
Figure 10. High-voltage activation of MPDEAs for reducing the hole
size (see Movie S1): (a) a photograph of a two-layer MPDEA
prototype and micrographs showing the hole contraction upon
activation; (b) a stepwise voltage ramp for activating a MPDEA and
the current leak across it; and (c) the voltage-induced contraction of
the through holes in a MPDEA.
Figure 11. Acoustic absorption spectrum of MPDEAs: (a) tunable
spectrums for a one-layer MPDEA and (b) tunable spectrums for a
two-layer MPDEA.
PEDOT:PSS electrode remains sub-megaohm, which is stable
enough for driving a DEA. Figure 4c−e shows the cyclic
activation of a dielectric elastomer actuator using square
voltage pulses between 0 and 3 kV. Given a constant relative
39948
Research Article
humidity, DEAs with PEDOT:PSS electrodes can repeatedly
actuate. However, the plasticized PEDOT:PSS electrodes dry
up and become stiff at a low relative humidity (e.g., 25%). This
stiffening effect of dried PEDOT:PSS greatly reduces the
dielectric elastomer actuation by nearly four times. This
observation agrees to the humidity-induced modulus change
reported by Lang et al.45 Interestingly, the electrodes soften
and the larger actuation restores upon re-exposure to high
relative humidity (e.g., 80%). This humidity effect on dielectric
elastomer actuation promises a novel kind of humidity sensor.
Next, we investigated the characteristics of inkjet-printed
PEDOT:PSS electrodes on dielectric elastomer membrane.
Figure 5a (second column) shows that an aqueous droplet of
pristine PEDOT:SS ink does not spread well on a VHB
substrate at a 44.54° contact angle. Inkjet printing of the
pristine aqueous ink cannot form a continuous wet film but
forms separated ink puddles on the VHB substrate. Here, we
formulated the ink in an optimized weight ratio of 40.78%
PEDOT:PSS ink, 4.5% Triton X-100, and 54.72% deionized
water (see table listing in Figure 5b). This optimized ink
spreads well (at an 11.5° contact angle) on the VHB substrate,
and it can be inkjet printed to form a continuous wet film,
which eventually evaporated to make a nanometric solid
coating of PEDOT:PSS (see Figure 5a, third column).
Figure 6a shows a printed dot of PEDOT:PSS ink with
diameter D = 38.10 μm and thickness 0.27 μm on the VHB
substrate. Figure 6b−e shows a continuous line can be formed
by printing at the following drop spacings: 10, 15, and 20 μm.
A closer print drop yields a thicker and wider line, but too
much ink droplets may reflow to distort the “straightness” of
line edges. Figure 7 shows a printed film obtained by printing
multiple lines with overlaps. A closer drop spacing, for
example, 10 or 15 μm, is required to obtain a continuous
film by allowing the reflow between a freshly printed wet drop
and a previously printed wet line that could have dried up a bit.
A thicker film obtained by printing at a closer drop spacing is
electrically more conductive but optically less clear (see Figure
7c,d).
Figure 7e shows a patch of printed film that was measured
with thicker edges due the coffee ring effect63 that happens
during the drying of a ink puddle. The measured sheet
resistance of a film printed at 20 μm drop spacing is less than
14.92 kΩ/□ measured normal to the print direction and less
than 1.34 kΩ/□ measured along the print direction. This
suggests a poorer electrical contact at the interface between the
print lines. After all, these films of printed PEDOT:PSS are
conductive enough to make for compliant electrodes of DEAs.
Stretchability of the inkjet-printed PEDOT:PSS thin film
can be tested on a standard dielectric elastomer actuator. This
dielectric elastomer actuator device consists of a prestretched
dielectric elastomer membrane (a VHB 4910 tape with three
times the radial prestretches) sandwiched between a pair of
circular PEDOT:PSS electrodes. Two types of inkjet-printed
PEDOT:PSS compliant electrodes are tested, namely, a thicker
film as obtained by printing at 15 μm drop spacing and a
thinner film as obtained by printing at 20 μm drop spacing. A
thicker film of inkjet-printed PEDOT:PSS is axially stiffer than
a thinner film.
Figure 8 shows the electrode area enlarging in a quadratic
trend with respect to increasing voltage up to an yield point
beyond which further actuation tapers. Thinner PEDOT:PSS
electrodes are axially softer than thicker ones. The DEA with
thinner PEDOT:PSS electrodes enlarges more than the one
DOI: 10.1021/acsami.8b12368
ACS Appl. Mater. Interfaces 2018, 10, 39942−39951
ACS Applied Materials & Interfaces
Figure 12. Performance comparison among transparent acoustic absorbers: (a) listing of material, resonator design, and optical and acoustic
performances; and (b) sound absorption spectrums.
with thicker electrodes when the same voltage was applied to
stretch the DEAs below the electrode yield point. However,
beyond the yield point, the PEDOT:PSS electrodes elongate
plastically and form necking.43 Interestingly, the DEA with
thicker electrodes can ultimately enlarge more beyond the
yield point. In short, the thicker PEDOT:PSS films (as
obtained from 15 μm drop space printing) are more
stretchable for driving the DEA. Figure 8d shows the
microridge formation in the released electrodes after 10 kV
activation (i.e., stretching) of the DEA. Figure 8f and Movie S1
show the ultimate dielectric elastomer actuation (e.g., D(V)/DI
= 1.14 at 9 kV) is limited by dielectric breakdown, which is
marked by a current surge.
Figure 9 shows that MPDEAs with inkjet-printed
PEDOT:PSS electrodes are slightly bluish. Whereas a single-
layer MPDEA is optically clear with close to 78.64% optical
transmittance, a two-layer MPDEA with double the number of
electrodes is less clear (of 61.8% transmittance for 550 nm
wavelength). The uneven bluish tone distribution suggests a
thickness variation in the printed film.
Figure 10 shows the electrical activation of MPDEAs
reducing the hole diameter 2a(V), smaller than the inactivated
one, 2ao. Two-layer MPDEA can sustain a higher driving
voltage up to 5.5 kV and thus reduces the hole diameter by
close to 15% (from 541.04 ± 25.36 μm diameter to 459.53 ±
20.40 μm diameter). When this MPDEA was activated under
44 MV/m nominal field, the power consumed was merely 1.14
mW or 3.62 W/m2. In comparison, the single-layer MPDEA
can only be driven up to 4 kV (for 10% hole diameter
contraction) due to premature electrical breakdown of the air
across shallow holes between opposite electrodes.
Moreover, these MPDEA devices with plasticized PE-
DOT:PSS electrodes are self-clearable and can survive a
premature breakdown upon voltage removal. As a result, the
ultimate breakdown voltage was raised, for example, from 4.5 V
for the first occurrence of breakdown to 5 kV for subsequent
occurrence. This self-healing of the devices happens because
the PEDOT:PSS electrodes surrounding the holes can be self-
cleared and thus the opposite electrodes next to each hole
become further apart. This self-clearing effect is similar to that
reported for nonperforated circular membrane DEAs using
other self-clearable compliant electrodes.24,28,64
Figure 11 shows the sound absorption spectrum of MPDEA-
based tunable acoustic absorbers. When not activated, a two-
39949
Research Article
layer MPDEA has the peak absorption at 1170 Hz resonant
frequency. Then, the bandwidth for above 80% sound
absorption is as broad as 444 Hz (from 836 to 1290 Hz).
When the two-layer MPDEA is activated with 6 kV, the
resonant frequency is shifted down by 15.2% to 992 Hz. In
comparison, a single-layer MPDEA shows a narrower
bandwidth and its 5 kV activation reduces the resonant
frequency by 18.5%.
4. BENCHMARK
So far, there are a few solutions of transparent acoustic
absorber, namely, translucent curtains (e.g., Gerriets Absorber
Light2), clear microperforated glass,3,9 and this work based on
microperforated dielectric elastomer absorber (MPDEA).
They all work on similar principle of resonant absorption. As
shown in Figure 12, their sound absorption bandwidths
however differ due to material, construction, and resonator
design.
Absorber light curtain is a 0.83 mm thick weave of polyester
fibers according to Gerriets.2 This flexible and translucent
acoustic absorber however needs a deep back cavity, for
example, a 150 mm depth to achieve at least 55% sound
absorption over a bandwidth close to 600 Hz. In comparison, a
5 mm thick glass panel with 0.5 mm diameter perforations can
achieve a similar bandwidth of sound absorption (for α > 55%)
even by using a slimmer back cavity of 25 mm according to
Fuchs and Zha.3 This slim design of a microperforated glass
acoustic absorber can save space for installation. Last but not
least, our MPDEA with flexible and stretchable membrane is
electrically tunable. Even when it is unpowered at the passive
state, it shows 800 Hz bandwidth (for α > 55%), which is
nearly 30% broader than those of the other two and electrically
tunable. A two-layered design of MPDEA shows a higher
maximum α of up to 97.4% at 934 Hz. However, it needs
further optimization to be optically clearer and physically
slimmer for installation to window glass.
In comparison, the previous MPDEA developed by our
group is larger in diameter (100 mm) and opaque owing to the
use of microwrinkled gold thin films as compliant electrodes.23
Its resonant frequency happens to be lower at 538.5 Hz, with a
larger diameter of back cavity, though the maximum peak
sound absorption coefficient is lower at 0.85. A 5 kV activation
can contract the hole size by 14.5% and this can shift down the
resonant frequency by 13.1%.
DOI: 10.1021/acsami.8b12368
ACS Appl. Mater. Interfaces 2018, 10, 39942−39951
ACS Applied Materials & Interfaces
5. CONCLUSIONS
This article presented a microperforated dielectric elastomer
absorber using inkjet-printed electrodes of plasticized
PEDOT:PSS thin films. This transparent acoustic absorber
can absorb mid-frequency sound while being optically clear. It
promises to make a quiet window glass and to prevent the
reverbration of indoor noises. Also formulated are soft
transparent compliant electrodes-based plasticized PE-
DOT:PSS with moderate stretchability for driving a dielectric
elastomer actuator and a tunable acoustic absorber membrane.
These transparent compliant electrodes are self-clearable and
durable for repeated use. However, modulus of plasticized
PEDOT:PSS is sensitive to humidity change. Although soft in
humid ambience of tropical country, plasticized PEDOT:PSS
becomes stiffened when dry. Further material design will be
needed to keep the electrodes soft even in dry ambience.
Together with dielectric elastomer, plasticized PEDOT:PSS
compliant electrodes are promising to tune acoustic meta-
surfaces56 while being equally useful for transparent generator
for acoustic energy harvesting65 and even tunable optical
devices.36,66
■
ASSOCIATED CONTENT
*
S Supporting Information
The Supporting Information is available free of charge on the
ACS Publications website at DOI: 10.1021/acsami.8b12368.
Fabrication of a tensile-test sample (Figure S1); nozzle
parameters for a Dimatix Material Cartridge (Figure S2);
experimental setup for measuring the inline optical
transmittance (Figure S3); experimental setup for
electromechanical activation (Figure S4) (PDF)
Voltage activation of dielectric elastomer device using
PEDOT:PSS nanometric thin-film compliant electrodes
(Movie S1) (MOV)
■
AUTHOR INFORMATION
Corresponding Author
*E-mail: mgklau@ntu.edu.sg.
ORCID
Gih-Keong Lau: 0000-0002-2065-076X
Author Contributions
M.S., Z.L., and G.-K.L. conceived the idea and designed the
study. M.S. contributed to all the material design and device
fabrication. Z.L. designed the experimental setup and
conducted the acoustic testing. M.S., Z.L., and G.-K.L. carried
out the data analysis. Z.L. and G.-K.L. derived the models. M.S.
and G.-K.L. wrote the manuscript. All the authors discussed
the results and revised the manuscript.
Notes
The authors declare no competing financial interest.
■
ACKNOWLEDGMENTS
This research was supported by Singapore Millennium
Foundation managed by Temasek Foundation Innovates.
The first author M.S. is grateful to Singapore Center for 3D
Printing (SC3DP) for supporting his Ph.D. scholarship.
■
REFERENCES
(1) Hernandez, P. For Restaurant Owners, Striking the Right Noise
Level is Key. The Boston Globes April 22, 2014. [Online] New
England Soundproofing. http://www.newenglandsoundproofing.
39950
Research Article
com/assets/files/wysiwyg/soundproofingrestaurant.pdf (accessed
July, 2018).
(2) Gerriets GmbH. Interior Acoustic Solutions. [Online] https://
www.gerriets.com/media/wysiwyg/downloads/acoustics/Gerriets-
EN-Interior-Acoustic-Solutions.pdf (accessed Jan 22, 2018).
(3) Fuchs, H.; Zha, X. Acrylic-glass Sound Absorbers in the Plenum
of the Deutscher Bundestag. Appl. Acoust. 1997, 51, 211−217.
(4) Kang, J.; Brocklesby, M. Feasibility of Applying Micro-perforated
Absorbers in Acoustic Window Systems. Appl. Acoust. 2005, 66, 669−
689.
(5) Kang, J. An Acoustic Window System with Optimum Ventilation
and Daylighting Performance. Noise & Vibration Worldwide 2006, 37,
9−17.
(6) Asdrubali, F.; Pispola, G. Properties of Transparent Sound-
absorbing Panels for Use in Noise Barriers. J. Acoust. Soc. Am. 2007,
121, 214−221.
(7) Wang, C.; Cheng, L.; Pan, J.; Yu, G. Sound Absorption of a
Micro-perforated Panel Backed by an Irregular-shaped Cavity. J.
Acoust. Soc. Am. 2010, 127, 238−246.
(8) Wang, C.; Huang, L. On the Acoustic Properties of Parallel
Arrangement of Multiple Micro-perforated Panel Absorbers with
Different Cavity Depths. J. Acoust. Soc. Am. 2011, 130, 208−218.
(9) Nocke, C. Optically Transparent Sound Absorber with Micro-
perforation. J. Acoust. Soc. Am. 2017, 141, 3872.
(10) Maa, D.-Y. Potential of Microperforated Panel Absorber. J.
Acoust. Soc. Am. 1998, 104, 2861−2866.
(11) Herrin, D.; Liu, J.; Seybert, A. Properties and Applications of
Microperforated Panels. Sound Vib. 2011, 45, 6−9.
(12) Pelrine, R. E.; Kornbluh, R. D.; Joseph, J. P. Electrostriction of
Polymer Dielectrics with Compliant Electrodes as a Means of
Actuation. Sens. Actuators, A 1998, 64, 77−85.
(13) Pelrine, R.; Kornbluh, R.; Pei, Q.; Joseph, J. High-speed
Electrically Actuated Elastomers with Strain greater than 100%.
Science 2000, 287, 836−839.
(14) Madden, J. D.; Vandesteeg, N. A.; Anquetil, P. A.; Madden, P.
G.; Takshi, A.; Pytel, R. Z.; Lafontaine, S. R.; Wieringa, P. A.; Hunter,
I. W. Artificial Muscle Technology: Physical Principles and Naval
Prospects. IEEE J. Ocean. Eng. 2004, 29, 706−728.
(15) Brochu, P.; Pei, Q. Advances in Dielectric Elastomers for
Actuators and Artificial Muscles. Macromol. Rapid Commun. 2010, 31,
10−36.
(16) Rosset, S.; Shea, H. R. Small, Fast, and Tough: Shrinking down
Integrated Elastomer Transducers. Appl. Phys. Rev. 2016, 3,
No. 031105.
(17) Maziz, A.; Concas, A.; Khaldi, A.; Stålhand, J.; Persson, N.-K.;
Jager, E. W. Knitting and Weaving Artificial Muscles. Sci. Adv. 2017, 3,
No. e1600327.
(18) Shintake, J.; Cacucciolo, V.; Floreano, D.; Shea, H. Soft Robotic
Grippers. Adv. Mater. 2018, 30, No. 1707035.
(19) Lu, Z.; Cui, Y.; Debiasi, M.; Zhao, Z. A Tunable Dielectric
Elastomer Acoustic Absorber. Acta Acust. Acust. 2015, 101, 863−866.
(20) Lu, Z.; Godaba, H.; Cui, Y.; Foo, C. C.; Debiasi, M.; Zhu, J. An
Electronically Tunable Duct Silencer using Dielectric Elastomer
Actuators. J. Acoust. Soc. Am. 2015, 138, EL236−EL241.
(21) Lu, Z.; Cui, Y.; Debiasi, M. Active Membrane-based Silencer
and its Acoustic Characteristics. Appl. Acoust. 2016, 111, 39−48.
(22) Dubois, P.; Rosset, S.; Niklaus, M.; Dadras, M.; Shea, H.
Voltage Control of the Resonance Frequency of Dielectric Electro-
active Polymer (DEAP) Membranes. J. Microelectromech. Syst. 2008,
17, 1072−1081.
(23) Lu, Z.; Shrestha, M.; Lau, G.-K. Electrically Tunable and
Broader-band Sound Absorption by using Micro-perforated Dielectric
Elastomer Actuator. Appl. Phys. Lett. 2017, 110, No. 182901.
(24) Low, S.-H.; Lau, G.-K. Bi-axially Crumpled Silver Thin-film
Electrodes for Dielectric Elastomer Actuators. Smart Mater. Struct.
2014, 23, No. 125021.
(25) Rothemund, P.; Morelle, X. P.; Jia, K.; Whitesides, G. M.; Suo,
Z. A Transparent Membrane for Active Noise Cancelation. Adv.
Funct. Mater. 2018, 28, No. 1800653.
DOI: 10.1021/acsami.8b12368
ACS Appl. Mater. Interfaces 2018, 10, 39942−39951
ACS Applied Materials & Interfaces
(26) Carpi, F.; Chiarelli, P.; Mazzoldi, A.; De Rossi, D. Electro-
mechanical Characterisation of Dielectric Elastomer Planar Actuators:
Comparative Evaluation of Different Electrode Materials and
Different Counterloads. Sens. Actuators, A 2003, 107, 85−95.
(27) Rosset, S.; Shea, H. R. Flexible and Stretchable Electrodes for
Dielectric Elastomer Actuators. Appl. Phys. A 2013, 110, 281−307.
(28) Yuan, W.; Hu, L.; Yu, Z.; Lam, T.; Biggs, J.; Ha, S. M.; Xi, D.;
Chen, B.; Senesky, M. K.; Grüner, G.; Pei, Q. Fault-Tolerant
Dielectric Elastomer Actuators using Single-Walled Carbon Nanotube
Electrodes. Adv. Mater. 2008, 20, 621−625.
(29) Shian, S.; Diebold, R. M.; McNamara, A.; Clarke, D. R. Highly
Compliant Transparent Electrodes. Appl. Phys. Lett. 2012, 101,
No. 061101.
(30) Shian, S.; Clarke, D. R. Electrically Tunable Window Device.
Opt. Lett. 2016, 41, 1289−1292.
(31) Keplinger, C.; Sun, J.-Y.; Foo, C. C.; Rothemund, P.;
Whitesides, G. M.; Suo, Z. Stretchable, transparent, ionic conductors.
Science 2013, 341, 984−987.
(32) Li, L.; Pan, L.; Ma, Z.; Yan, K.; Cheng, W.; Shi, Y.; Yu, G. All
Inkjet-Printed Amperometric Multiplexed Biosensors Based on
Nanostructured Conductive Hydrogel Electrodes. Nano Lett. 2018,
18, 3322−3327.
(33) Lett, J. K. Hydrogel Electrodes: What you should know about
Hydrogel Electrodes. TheraSigma 2013 [Online] http://www.
therasigma.com/wpcontent/uploads/Hydrogel-Electrodes-White-
Paper.pdf (accessed June, 2018).
(34) Kosierkiewicz, T. A. Dry and Flexible Elastomer Electrodes
Outperform Similar Hydrogel and Ag/AgCl Electrodes. In Medical
Measurements and Applications Proceedings (MeMeA), 2013 IEEE
International Symposium on; IEEE, 2013; pp 306−308.
(35) Christianson, C.; Goldberg, N. N.; Deheyn, D. D.; Cai, S.;
Tolley, M. T. Translucent Soft Robots Driven by Frameless Fluid
Electrode Dielectric Elastomer Actuators. Sci. Robotics 2018, 3,
No. eaat1893.
(36) Carpi, F.; Frediani, G.; Turco, S.; De Rossi, D. Bioinspired
Tunable Lens with Muscle-like Electroactive Elastomers. Adv. Funct.
Mater. 2011, 21, 4152−4158.
(37) Lau, G.-K.; Tan, D. D.-T.; La, T.-G. Large Axial Actuation of
Pre-stretched Tubular Dielectric Elastomer and Use of Oil
Encapsulation to Enhance Dielectric Breakdown Strength. Smart
Mater. Struct. 2015, 24, No. 045025.
(38) Nardes, A.; Kemerink, M.; Janssen, R. Anisotropic Hopping
Conduction in Spin-coated PEDOT: PSS Thin Films. Phys. Rev. B
2007, 76, No. 085208.
(39) Liu, Y.; Cui, T.; Varahramyan, K. All-polymer Capacitor
Fabricated with Inkjet Printing Technique. Solid-State Electron. 2003,
47, 1543−1548.
(40) Sirringhaus, H.; Kawase, T.; Friend, R.; Shimoda, T.;
Inbasekaran, M.; Wu, W.; Woo, E. High-resolution Inkjet Printing
of All-polymer Transistor Circuits. Science 2000, 290, 2123−2126.
(41) Burns, S. E.; Cain, P.; Mills, J.; Wang, J.; Sirringhaus, H. Inkjet
Printing of Polymer Thin-film Transistor Circuits. MRS Bull. 2003,
28, 829−834.
(42) Eom, S. H.; Senthilarasu, S.; Uthirakumar, P.; Yoon, S. C.; Lim,
J.; Lee, C.; Lim, H. S.; Lee, J.; Lee, S.-H. Polymer Solar Cells based on
Inkjet-printed PEDOT: PSS Layer. Org. Electron. 2009, 10, 536−542.
(43) Lipomi, D. J.; Lee, J. A.; Vosgueritchian, M.; Tee, B. C.-K.;
Bolander, J. A.; Bao, Z. Electronic Properties of Transparent
Conductive Films of PEDOT: PSS on Stretchable Substrates. Chem.
Mater. 2012, 24, 373−382.
(44) Vosgueritchian, M.; Lipomi, D. J.; Bao, Z. Highly Conductive
and Transparent PEDOT: PSS Films with a Fluorosurfactant for
Stretchable and Flexible Transparent Electrodes. Adv. Funct. Mater.
2012, 22, 421−428.
(45) Lang, U.; Naujoks, N.; Dual, J. Mechanical Characterization of
PEDOT: PSS Thin Films. Synth. Met. 2009, 159, 473−479.
(46) Bozlar, M.; Punckt, C.; Korkut, S.; Zhu, J.; Chiang Foo, C.;
Suo, Z.; Aksay, I. A. Dielectric Elastomer Actuators with Elastomeric
Electrodes. Appl. Phys. Lett. 2012, 101, No. 091907.
39951
Research Article
(47) Michel, S.; Zhang, X. Q.; Wissler, M.; Löwe, C.; Kovacs, G. A
Comparison between Silicone and Acrylic Elastomers as Dielectric
Materials in Electroactive Polymer Actuators. Polym. Int. 2010, 59,
391−399.
(48) Yoon, S.-S.; Khang, D.-Y. Roles of Nonionic Surfactant
Additives in PEDOT: PSS Thin Films. J. Phys. Chem. C 2016, 120,
29525−29532.
(49) Greco, F.; Zucca, A.; Taccola, S.; Menciassi, A.; Fujie, T.;
Haniuda, H.; Takeoka, S.; Dario, P.; Mattoli, V. Ultra-thin Conductive
Free-standing PEDOT/PSS Nanofilms. Soft Matter 2011, 7, 10642−
10650.
(50) Lau, G.-K.; Heng, K.-R.; Ahmed, A. S.; Shrestha, M. Dielectric
Elastomer Fingers for Versatile Grasping and Nimble Pinching. Appl.
Phys. Lett. 2017, 110, No. 182906.
(51) Plante, J.-S.; Dubowsky, S. Large-scale Failure Modes of
Dielectric Elastomer Actuators. Int. J. Solids Struct. 2006, 43, 7727−
7751.
(52) Lau, G.-K.; La, T.-G.; Foong, E. S.-W.; Shrestha, M. Stronger
Multilayer Acrylic Dielectric Elastomer Actuators with Silicone Gel
Coatings. Smart Mater. Struct. 2016, 25, No. 125006.
(53) Pimpin, A.; Suzuki, Y.; Kasagi, N. Microelectrostrictive
Actuator with Large Out-of-plane Deformation for Flow-control
Application. J. Microelectromech. Syst. 2007, 16, 753−764.
(54) Shrestha, M.; Asundi, A.; Lau, G.-K. Smart Window Based on
Electric Unfolding of Microwrinkled TiO2 Nanometric Films. ACS
Photonics 2018, 5, 3255−3262.
(55) Ginn, K. Architectural Acoustics; Brüel & Kjaer: Naerum,
Denmark, 1978; pp 56−58.
(56) Ma, G.; Yang, M.; Xiao, S.; Yang, Z.; Sheng, P. Acoustic
Metasurface with Hybrid Resonances. Nat. Mater. 2014, 13, No. 873.
(57) Dimatix Materials Printer DMP-2800 Series User Manual;
FUJIFILM Dimatix, Inc., 2015.
(58) Lau, G.-K.; Shrestha, M. Ink-jet Printing of Micro-Elelectro-
Mechanical Systems (MEMS). Micromachines 2017, 8, No. 194.
(59) de Gans, B.-J.; Duineveld, P. C.; Schubert, U. S. Inkjet Printing
of Polymers: State of the Art and Future Developments. Adv. Mater.
2004, 16, 203−213.
(60) Chen, C.-T.; Wu, K.-H.; Lu, C.-F.; Shieh, F. An Inkjet Printed
Stripe-type Color Filter of Liquid Crystal Display. J. Micromech.
Microeng. 2010, 20, No. 055004.
(61) Chung, J.; Blaser, D. Transfer Function Method of Measuring
In-duct Acoustic Properties. II. Experiment. J. Acoust. Soc. Am. 1980,
68, 914−921.
(62) Nardes, A. M.; Kemerink, M.; De Kok, M.; Vinken, E.;
Maturova, K.; Janssen, R. Conductivity, Work Function, and
Environmental Stability of PEDOT: PSS Thin Films Treated with
Sorbitol. Org. Electron. 2008, 9, 727−734.
(63) Soltman, D.; Subramanian, V. Inkjet-printed Line Morpholo-
gies and Temperature Control of the Coffee Ring Effect. Langmuir
2008, 24, 2224−2231.
(64) La, T.-G.; Lau, G.-K. Inhibiting Electro-thermal Breakdown of
Acrylic Dielectric Elastomer Actuators by Dielectric Gel Coating.
Appl. Phys. Lett. 2016, 108, No. 012903.
(65) Yang, J.; Chen, J.; Liu, Y.; Yang, W.; Su, Y.; Wang, Z. L.
Triboelectrification-based Organic Film Nanogenerator for Acoustic
Energy Harvesting and Self-powered Active Acoustic Sensing. ACS
Nano 2014, 8, 2649−2657.
(66) Maffli, L.; Rosset, S.; Ghilardi, M.; Carpi, F.; Shea, H. Ultrafast
All-Polymer Electrically Tunable Silicone Lenses. Adv. Funct. Mater.
2015, 25, 1656−1665.
DOI: 10.1021/acsami.8b12368
ACS Appl. Mater. Interfaces 2018, 10, 39942−39951